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Abstract The integration of dissimilar materials into heterostructures is a mainstay of modern materials science and technology. An alternative strategy of joining components with different electronic structure involves mixed‐dimensional heterostructures, that is, architectures consisting of elements with different dimensionality, for example, 1D nanowires and 2D plates. Combining the two approaches can result in hybrid architectures in which both the dimensionality and composition vary between the components, potentially offering even larger contrast between their electronic structures. To date, realizing such heteromaterials mixed‐dimensional heterostructures has required sequential multi‐step growth processes. Here, it is shown that differences in precursor incorporation rates between vapor–liquid–solid growth of 1D nanowires and direct vapor–solid growth of 2D plates attached to the wires can be harnessed to synthesize heteromaterials mixed‐dimensional heterostructures in a single‐step growth process. Exposure to mixed GeS and GeSe vapors produces GeS_1−xSe_xvan der Waals nanowires whose S:Se ratio is considerably larger than that of attached layered plates. Cathodoluminescence spectroscopy on single heterostructures confirms that the bandgap contrast between the components is determined by both composition and carrier confinement. These results demonstrate an avenue toward complex heteroarchitectures using single‐step synthesis processes.